Ab initio study of effects of Al and Y co-doping on destabilizing of MgH2

First-principles calculations based on density functional theory (DFT) were performed to study the destabilizing mechanism of co-doped MgH2 with Al and Y. From the minimization of total electronic energy, the preferential positions of dopants are determined. The calculated formation enthalpy and substitution enthalpy show that incorporation of Al combined with Y atoms into MgH2 is energetically favorable relative to Al doping alone. Due to strong interaction of the dopant Y with Mg and Al, the hydrogen dissociation energy and the dehydrogenation enthalpy are both reduced, indicating that the synergetic effect of Al and Y on destabilizing the MgH2 is superior to that of Al doping. The electronic structures show that the breakage of Mg–H bond is much easier in co-doped case, because of the conduction band shift below the Fermi level and the hybridization of dopants with Mg atoms, which effectively decrease the hybridization between Mg and H.